通过MnO2电催化剂将水氧化为分子氧的pH取决活性机制
Toshihiro Takashima1, Kazuhito Hashimoto, Ryuhei Nakamura
1Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Tokyo 113-8656, Japan.
Journal of the American Chemical Society
|December 31, 2011
概括
由于不稳定的3+ (Mn3+),氧化物在中性pH下是氧化水的不良催化剂. 通过可控反应稳定Mn3+是开发有效的催化剂的关键,用于中性水氧化.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 氧化是有效的电催化剂,在性条件下氧化水.
- 它们的效率在中性pH下显著下降,阻碍了更广泛的应用.
- 了解pH依赖机制对于开发改进的催化剂至关重要.
研究的目的:
- 研究氧化物电催化剂对水氧化的pH依赖活性背后的机制.
- 为了确定涉及到水氧化过程的中间物种,在一系列的pH值范围内.
- 阐明氧化状态在催化效率中的作用.
主要方法:
- 使用UV-VIS光谱电化学检测来监测中间物种.
- 在配氧化电极上使用了分层的氧化纳米粒子 (δ-MnO2).
- 酸盐被用作探针分子来识别表面物种.
主要成果:
- 吸收在510nm的急剧增加,归因于Mn(3+),与氧气演变相关.
- 水氧化的开始潜力从pH 4到8保持不变,但在pH 8以上变为负.
- 3+) 形成的pH依赖反映了水的氧化活性,确定3+) 作为水的氧化前体.
结论:
- 由于在pH值<9的不成比例,Mn3+的不稳定性解释了氧化物在中性pH值的低活性.
- 在性条件下稳定Mn(3+) 是通过对比实现的.
- 控制Mn ((3+) 不成比例和占比对于开发高效的中性pH水氧化催化剂至关重要.
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